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Rephasing and non-rephasing two-dimensional coherent spectra map the anti-crossing associated with normal-mode splitting in a semiconductor microcavity. For a 12-meV detuning range near zero detuning, it is observed that there are two diagonal featur es related to the intra-action of exciton-polariton branches and two off-diagonal features related to coherent interaction between the polaritons. At negative detuning, the lineshape properties of the diagonal intra-action features are distinguishable and can be associated with cavity-like and exciton-like modes. A biexcitonic companion feature is observed, shifted from the exciton feature by the biexciton binding energy. Closer to zero detuning, all features are enhanced and the diagonal intra-action features become nearly equal in amplitude and linewidth. At positive detuning the exciton- and cavity-like characteristics return to the diagonal intra-action features. Off-diagonal interaction features exhibit asymmetry in their amplitudes throughout the detuning range. The amplitudes are strongly modulated (and invert) at small positive detuning, as the lower polariton branch crosses the bound biexciton energy determined from negative detuning spectra.
Films of the topological insulator Bi2Se3 are grown by molecular beam epitaxy with in-situ reflection high-energy electron diffraction. The films are shown to be high-quality by X-ray reflectivity and diffraction and atomic-force microscopy. Quantum interference control of photocurrents is observed by excitation with harmonically related pulses and detected by terahertz radiation. The injection current obeys the expected excitation irradiance dependence, showing linear dependence on the fundamental pulse irradiance and square-root irradiance dependence of the frequency-doubled optical pulses. The injection current also follows a sinusoidal relative-phase dependence between the two excitation pulses. These results confirm the third-order nonlinear optical origins of the coherently controlled injection current. Experiments are compared to a tight-binding band structure to illustrate the possible optical transitions that occur in creating the injection current.
Photoluminescence spectra of YVO$_{4}$:Eu$^{3+}$ nanoparticles are presented,with and without the attachment of of organic linker molecules that are proposed for linking to biomolecules. YVO$_{4}$:Eu$^{3+}$ nanoparticles with 5% dopant concentration were synthesized by wet chemical synthesis. X-ray diffraction and transmission electron microscopy show the expected wakefieldite structure of tetragonal particles with an average size of 17 nm. Fourier-transform infrared spectroscopy determines that metal-carboxylate coordination is successful in replacing the native metal-hydroxyl bonds with three organic linkers, namely benzoic acid, 3-nitro 4-chloro-benzoic acid and 3,4-dihydroxybenzoic acid, in separate treatments. UV-excitation photoluminescence spectra show that the position and intensity of dominant $^{5}D_{0}-^{7}F_{2}$ electric-dipole transition at 619 nm is unaffected by the benzoic acid and 3-nitro 4-chloro-benzoic acid treatments. Attachment of the 3,4-dihydroxybenzoic acid produces an order-of-magnitude quenching of the photoluminescence, due to the presence of high-frequency modes in the linker. Ratios of the dominant electric- and magnetic-dipole transitions confirm infrared measurements, which indicate that the bulk crystal of the nanoparticle is unchanged by all three treatments.
Collinear phase-matched optical rectification is studied in ZnGeP$_{2}$ pumped with near-infrared light. The pump-intensity dependence is presented for three crystal lengths (0.3, 1.0 and 3.0 mm) to determine the effects of linear optical absorption, nonlinear optical absorption and terahertz free-carrier absorption on the generation. Critical parameters such as the coherence length (for velocity matching), dispersion length (for linear pulse broadening) and nonlinear length (for self-phase modulation) are determined for this material. These parameters provide insight into the upper limit of pulse intensity and crystal length required to generate intense terahertz pulse without detriment to the pulse shape. It is found that for 1-mm thick ZnGeP$_{2}$(012), pumped at 1.28 micron with intensity of ~15 GW/cm2 will produce intense undistorted pulses, whereas longer crystals or larger intensities modify the pulse shape to varying degrees. Moreover, phase-matching dispersion maps are presented for the terahertz generation over a large tuning range (1.1-2.4 micron) in longer (3 mm) crystal, demonstrating the phase-matching bandwidth and phase mismatch that leads to fringing associated with multi-pulse interference. All observed results are simulated numerically showing good qualitative agreement.
We propose the use of a silicon-core optical fiber for terahertz (THz) waveguide applications. Finite-difference time-domain simulations have been performed based on a cylindrical waveguide with a silicon core and silica cladding. High-resistivity si licon has a flat dispersion over a 0.1 - 3 THz range, making it viable for propagation of tunable narrowband CW THz and possibly broadband picosecond pules of THz radiation. Simulations show the propagation dynamics and the integrated intensity, from which transverse mode profiles and absorption lengths are extraced. It is found that for 140 - 250 micron core diameters the mode is primarily confined to the core, such that the overall absorbance is only slightly less than in bulk polycrystalline silicon.
The angular dependence of terahertz (THz) emission from birefringent crystals can differ significantly from that of cubic crystals. Here we consider optical rectification in uniaxial birefringent materials, such as chalcopyrite crystals. The analysis is verified in (110)-cut ZnGeP_2 and compared to (zincblende) GaP. Although the crystals share the same nonzero second-order tensor elements, the birefringence in chalcopyrite crystals cause the pump pulse polarization to evolve as it propagates through the crystal, resulting in a drastically different angular dependence in chalcopyrite crystals. The analysis is extended to {012}- and {114}-cut chalcopyrite crystals and predicts more efficient conversion for the {114} crystal cut over the {012}- and {110}-cuts.
We study the coherent light-matter interactions of GaAs quantum wells associated with excitons, biexcitons and many-body effects. For most polarization configurations, excitonic features dominate the phase-resolved two-dimensional Fourier-transform ( 2DFT) spectra and have dispersive lineshapes, indicating the presence of many-body interactions. For cross-linear excitation, excitonic features become weak and absorptive due to the strong suppression of many-body effects; a result that can not be directly determined in transient four-wave mixing experiments. The biexcitonic features do not weaken for cross-polarized excitation and thus are more important.
A combination of spatial interference patterns and spectral interferometry are used to find the global phase for non-collinear two-dimensional Fourier-transform (2DFT) spectra. Results are compared with those using the spectrally resolved transient a bsorption (STRA) method to find the global phase when excitation is with co-linear polarization. Additionally cross-linear polarized 2DFT spectra are correctly phased using the all-optical technique, where the SRTA is not applicable.
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